Molecularly-Enhanced Heterogeneous Catalysts for CO₂ Electroconversion

Abstract

Electrochemical CO2 reduction reaction (CO2RR) which can convert CO2 to fuels and feedstocks addresses the needs for carbon neutrality. Production of hydrocarbons and oxygenates is in sight; yet it remains a challenge for selective and efficient electrosynthesis. Introducing molecular approaches to CO2RR electrocatalysts can enhance product selectivity and catalytic activity by leveraging the interplay between heterogeneous and homogeneous catalysts. Here, I will present our recent efforts to develop molecularly-enhanced CO2RR electrocatalysts. First, we studied ionomers which control the microenvironment of gas diffusion electrode. We unveil how side chains and ionic groups in ionomers affect CO2/H2O ratio and CO2RR of Cu electrocatalysts. Second, we introduce how we harness metal-organic frameworks (MOFs) for CO2RR. This work provides the guidelines to understand the reconstruction of MOFs. Perspective will be discussed in conclusion.